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We report excellent electrostrain properties of (1 − x)BaTiO3–xSrSnO3 (BSTS) Pb‐free electroceramics (0 ≤ x ≤ 0.15), as well as the corresponding structural, dielectric, and ferroelectric properties. A tailored phase diagram of the pseudo‐binary solid solution of BaTiO3–SrSnO3, which exhibits a nearly composition‐independent orthorhombic–tetragonal polymorphic phase boundary close to room temperature,...